For the majority of higher plants, silicon (Si) is considered a beneficial element because of the various favorable effects of Si accumulation in plants that have been revealed, including the alleviation of metal(loid) toxicity. The accumulation of non-degradable metal(loid)s in the environment strongly increased in the last decades by intensified industrial and agricultural production with negative consequences for the environment and human health. Phytoremediation, i.e., the use of plants to extract and remove elemental pollutants from contaminated soils, has been commonly used for the restoration of metal(loid)-contaminated sites. In our viewpoint article, we briefly summarize the current knowledge of Si-mediated alleviation of metal(loid) toxicity in plants and the potential role of Si in the phytoremediation of soils contaminated with metal(loid)s. In this context, a special focus is on metal(loid) accumulation in (soil) phytoliths, i.e., relatively stable silica structures formed in plants. The accumulation of metal(loid)s in phytoliths might offer a promising pathway for the long-term sequestration of metal(loid)s in soils. As specific phytoliths might also represent an important carbon sink in soils, phytoliths might be a silver bullet in the mitigation of global change. Thus, the time is now to combine Si/phytolith and phytoremediation research. This will help us to merge the positive effects of Si accumulation in plants with the advantages of phytoremediation, which represents an economically feasible and environmentally friendly way to restore metal(loid)-contaminated sites.